Exposure error in studies of ambient air pollution and health that use city-wide measures of exposure may be substantial for pollutants that exhibit spatiotemporal variability. Alternative spatiotemporal metrics of exposure for traffic-related and regional pollutants were applied in a time-series study of ambient air pollution and cardiorespiratory emergency department visits in Atlanta, GA, USA. Exposure metrics included daily central site monitoring for particles and gases; daily spatially refined ambient concentrations obtained from regional background monitors, local-scale dispersion, and hybrid air quality models; and spatially refined ambient exposures from population exposure models. Health risk estimates from Poisson models using the different exposure metrics were compared. We observed stronger associations, particularly for traffic-related pollutants, when using spatially refined ambient concentrations compared with a conventional central site exposure assignment approach. For some relationships, estimates of spatially refined ambient population exposures showed slightly stronger associations than corresponding spatially refined ambient concentrations. Using spatially refined pollutant metrics, we identified socioeconomic disparities in concentration-response functions that were not observed when using central site data. In some cases, spatially refined pollutant metrics identified associations with health that were not observed using measurements from the central site. Complexity and challenges in incorporating modeled pollutant estimates in time-series studies are discussed.